WO2010100906A1 - 高分子電解質型燃料電池用ガスケット - Google Patents

高分子電解質型燃料電池用ガスケット Download PDF

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Publication number
WO2010100906A1
WO2010100906A1 PCT/JP2010/001439 JP2010001439W WO2010100906A1 WO 2010100906 A1 WO2010100906 A1 WO 2010100906A1 JP 2010001439 W JP2010001439 W JP 2010001439W WO 2010100906 A1 WO2010100906 A1 WO 2010100906A1
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WO
WIPO (PCT)
Prior art keywords
seal
gasket
mountain
shaped portion
fuel cell
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2010/001439
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English (en)
French (fr)
Japanese (ja)
Inventor
山本曜子
松本敏宏
森本隆志
吉村光生
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Panasonic Corp
Original Assignee
Panasonic Corp
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Panasonic Corp filed Critical Panasonic Corp
Priority to EP10748505.4A priority Critical patent/EP2405516B1/de
Priority to JP2010546161A priority patent/JP4800443B2/ja
Priority to US13/254,244 priority patent/US8962212B2/en
Publication of WO2010100906A1 publication Critical patent/WO2010100906A1/ja
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
    • H01M8/0263—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant having meandering or serpentine paths
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0267—Collectors; Separators, e.g. bipolar separators; Interconnectors having heating or cooling means, e.g. heaters or coolant flow channels
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0273—Sealing or supporting means around electrodes, matrices or membranes with sealing or supporting means in the form of a frame
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0276—Sealing means characterised by their form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0286—Processes for forming seals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
    • H01M8/242—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes comprising framed electrodes or intermediary frame-like gaskets
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2465—Details of groupings of fuel cells
    • H01M8/2483—Details of groupings of fuel cells characterised by internal manifolds
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M2008/1095—Fuel cells with polymeric electrolytes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/028—Sealing means characterised by their material
    • H01M8/0284—Organic resins; Organic polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2465—Details of groupings of fuel cells
    • H01M8/247—Arrangements for tightening a stack, for accommodation of a stack in a tank or for assembling different tanks
    • H01M8/248—Means for compression of the fuel cell stacks
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the present invention relates to a fuel cell used for a portable power source, a power source for an electric vehicle, a home cogeneration system, or the like, and more particularly, to a gasket for a polymer electrolyte fuel cell using a polymer electrolyte.
  • a fuel cell using a polymer electrolyte generates electric power and heat simultaneously by electrochemically reacting a fuel gas containing hydrogen and an oxidant gas containing oxygen such as air.
  • This fuel cell basically includes a polymer electrolyte membrane that selectively transports hydrogen ions and a pair of electrodes formed on both sides of the polymer electrolyte membrane, that is, an anode and a cathode.
  • These electrodes are mainly composed of carbon powder supporting a platinum group metal catalyst, and have both a gas permeability and an electronic conductivity disposed on the outer surface of the catalyst layer formed on the surface of the polymer electrolyte membrane and the catalyst layer. It has a gas diffusion layer.
  • An assembly in which the polymer electrolyte membrane and the electrode (including the gas diffusion layer) are integrally joined together is called an electrolyte membrane electrode assembly (hereinafter referred to as “MEA”).
  • MEA electrolyte membrane electrode assembly
  • conductive separators for mechanically sandwiching and fixing the MEAs and electrically connecting adjacent MEAs to each other in series are arranged.
  • a gas flow path for supplying a reaction gas such as a fuel gas or an oxidant gas to each electrode and carrying away generated water or surplus gas is formed at a portion in contact with the MEA.
  • a gas flow path can be provided separately from the separator, but a system in which a groove is provided on the surface of the separator to form a gas flow path is generally used.
  • a structure in which the MEA is sandwiched between the pair of separators is referred to as a “single cell module”.
  • the supply of the reaction gas to the gas flow path formed between each separator and the MEA, the reaction gas from the gas flow path, and the discharge of the generated water are performed at the edge of at least one separator of the pair of separators. This is done by providing through holes called manifold holes, communicating the inlets and outlets of the respective gas flow paths with these manifold holes, and distributing the reaction gas from each manifold hole to each gas flow path.
  • the portion where the electrodes in the MEA are formed that is, the outer periphery of the power generation region, so that the fuel gas or oxidant gas supplied to the gas flow path does not leak to the outside or the two kinds of gases are mixed with each other
  • a gas sealing material or a gasket is disposed as a sealing member so as to surround.
  • a cooling section for flowing cooling water is provided for every 1 to 3 cells.
  • These MEAs, separators, and cooling units are alternately stacked, and after stacking 10 to 200 cells, end plates are arranged at the respective end portions of these cells via current collector plates and insulating plates. These cells are sandwiched between end plates and fixed from both ends with fastening bolts (rods) or the like in a general laminated battery (fuel cell stack) structure.
  • fastening method a method of passing through a through hole formed in the edge of each separator and fastening with a fastening bolt, or a method of fastening the whole laminated battery with a metal belt over an end plate is common.
  • Patent Document 2 as shown in FIG. 9 as an example of a gasket that responds to a request for low reaction force, can prevent a lip from falling, and can maintain a sealing property even with a minute unevenness or a step on a mating surface.
  • a two-stage gasket 201 has been proposed.
  • the gasket 201 is integrally molded and attached to one of the two members facing each other, and the seal lip 202 provided by integrally molding the gasket 201 in close contact with the other is crushed in order to reduce the reaction force. Has a small shape.
  • a seal portion in a fuel cell gasket, has an inner seal formed of a lip having a substantially triangular cross section protruding in both directions, and a substantially triangular cross section that is located outside the inner seal and protrudes in both directions. It has an outer seal formed by a lip, and the inner seal and the outer seal are connected by an annular connecting portion.
  • Patent Document 4 is configured such that a seal lip having a bi-directional sealing property is provided in a seal portion, and a sealing lip having a uni-directional sealing property is provided on one side or both sides of the seal lip. With such a configuration, it is possible to meet the demand for low reaction force, maintain the sealing function even if the lip collapses, and even if there are minute irregularities or steps on the mating surface The sealing function can be maintained.
  • Patent Document 5 a pair of interval restricting portions each having a quadrilateral cross section is disposed on the periphery of the rubber sheet, and a lip line portion having a chevron or triangular cross section is disposed between the pair of interval restricting portions.
  • the pair of gap regulating portions controls the dimensions so that the lip line portion performs desired compression deformation.
  • rubber as a gasket body made of a rubber-like elastic material has a seal lip portion and is formed in a cross-sectional triangle shape or a mountain shape, and has a bead-like seal lip (also referred to as a bead).
  • a flat seal structure is disclosed.
  • the surface pressure peak value of the gasket body can be adjusted even if the bonding position of the resin film on both sides is slightly shifted left and right.
  • an apparatus that can prevent the decrease in the temperature.
  • an object of the present invention is to solve the above-mentioned problems, and in a polymer electrolyte fuel cell, to provide a double seal structure capable of reliably ensuring sealing performance, and at the same time, there is a conflicting requirement of the stack. It is an object of the present invention to provide a gasket for a polymer electrolyte fuel cell that can realize a reduction in size and a lower fastening force.
  • the present invention is configured as follows.
  • the gasket for a polymer electrolyte fuel cell includes a membrane electrode assembly, seal members disposed on both outer surfaces of the membrane electrode assembly, the membrane electrode assembly, A single battery module having a pair of separators sandwiching a seal member is laminated to form a laminate, and assembled by being clamped by a fastening member via a pair of end plates disposed at both ends of the laminate.
  • the seal member is integrally formed on the outer peripheral portions of the front and back surfaces of the membrane electrode assembly, As the seal member, two rows of seal lips each having sealing properties are continuously provided in parallel in the plane, and at least the outer seal lip of the two rows of seal lips is on the lower mountain-shaped portion.
  • a polymer electrolyte fuel characterized in that the upper mountain-shaped portion is integrally formed by overlapping, and the curvature radius of the vertex of the lower mountain-shaped portion is larger than the curvature radius of the vertex of the upper mountain-shaped portion
  • a battery gasket is provided.
  • the radius of curvature of the vertex of the lower chevron-shaped portion and R 1 the radius of curvature of the vertex of the upper chevron-shaped portion when the R 2, and the radius of curvature R 1 wherein the correlation between the radius of curvature R 2, R 1 ⁇ 0.5 ⁇ R 2 is satisfied
  • the height of the portion between the two rows of seal lips is formed to be lower than the height at which the two rows of seal lips are tightened by the separators on the front and back surfaces of the membrane electrode assembly.
  • the apex angle of the lower mountain-shaped portion and the apex angle of the upper mountain-shaped portion are 18 ° or more, and are orthogonal to the thickness direction of the two rows of seal lips and
  • the dimension in the thickness direction from the outer peripheral surface of the membrane electrode assembly to the apex of the upper mountain-shaped portion is 60% or less with respect to the full width along the direction orthogonal to the extending direction of the two rows of seal lips.
  • the upper mountain-shaped portion and the lower mountain-shaped portion are both circular in cross section near the apex,
  • the upper mountain-shaped portion is more easily deformed than the vertex portion of the lower mountain-shaped portion so that the vertex portion of the upper mountain-shaped portion comes into contact with the separator and is greatly elastically deformed.
  • the lower mountain-shaped portion is a seal area expanding portion that enlarges the seal area between the separator by deforming the apex portion of the lower mountain-shaped portion after the easily deformable portion is greatly elastically deformed.
  • a gasket for a polymer electrolyte fuel cell according to any one of the first to third aspects is provided.
  • a space-saving and low reaction force double seal can be realized.
  • FIG. 1 is an exploded perspective view of a fuel cell stack according to a first embodiment of the present invention.
  • FIG. 2A is a plan view schematically showing the MEA and gasket structure of the fuel cell stack of FIG. 2B is a plan view showing a fuel gas gasket structure of the MEA adjacent to the fuel gas flow channel groove of the separator 10A of the fuel cell stack of FIG.
  • FIG. 3A is a partial cross-sectional view of a gasket structure according to a conventional example (partial cross-sectional view of a gasket structure according to a conventional example with respect to a portion similar to the line AA in FIG. 2A); 3B is a cross-sectional view taken along line AA of FIG. 2A of the gasket structure of the fuel cell stack according to the first embodiment of the present invention; 4A is a partial cross-sectional view of a double seal structure of an MEA and a pair of separators using the conventional gasket (a double seal structure according to a conventional example of the same portion as the line AA in FIG. 2A). Is a diagram of a state in which a gasket and a separator are virtually assembled, FIG.
  • FIG. 4B is a partial cross-sectional view of a double seal structure of a MEA using a gasket of the fuel cell stack according to the first embodiment and a pair of separators (part of the double seal structure taken along line AA in FIG. 2A). It is a sectional view), and is a diagram of a state where a gasket and a separator are virtually assembled
  • FIG. 4C is a graph showing a comparison between the seal reaction force in the conventional gasket structure and the seal reaction force in the gasket structure of the first embodiment of the present invention
  • FIG. 4D is a partial cross-sectional explanatory view showing a comparison in dimensions between the gasket structure of the conventional example and the gasket structure of the first embodiment, FIG.
  • FIG. 4E is a partial cross-sectional view of the double seal structure of the MEA and the pair of separators using the gasket of the conventional example at the time of fastening (according to the conventional example of the same part as the AA line of FIG. 2A).
  • a partial cross-sectional view of a double seal structure FIG. 4F is a partial cross-sectional view of a double seal structure of a MEA that uses the gasket of the fuel cell stack according to the first embodiment and a pair of separators at the time of fastening (double line along line AA in FIG. 2A).
  • FIG. 5A is a partial cross-sectional view showing a modification of the first embodiment, FIG.
  • FIG. 5B is a partial cross-sectional view showing another modification of the gasket of the first embodiment
  • FIG. 6A is a partial cross-sectional view of the gasket structure according to the second embodiment of the present invention, in a state where the MEA and the separator are virtually assembled
  • FIG. 6B is a partial cross-sectional view of the gasket structure according to the second embodiment of the present invention at the time of fastening
  • FIG. 7A is a partial cross-sectional view of a gasket structure according to a third embodiment of the present invention, and is a view of a state where an MEA and a separator are virtually assembled
  • FIG. 7B is a partial cross-sectional view of the gasket structure according to the third embodiment of the present invention at the time of fastening
  • FIG. 8 is a partial cross-sectional view showing an example of the embodiment in Patent Document 1.
  • FIG. 9 is a partial cross-sectional view showing an example of the embodiment in Patent Document 2.
  • 10A is an enlarged cross-sectional view of a part of the gasket structure of the fuel cell stack according to the first embodiment of FIG. 3B;
  • FIG. 10B is an enlarged cross-sectional view in a state where the gasket of FIG. 10A is pressed against the separator,
  • FIG. 11A is an enlarged cross-sectional view of a state immediately before the conventional one-stage lip gasket is pressed against the separator;
  • FIG. 11B is an enlarged cross-sectional view of a state in which the conventional one-stage lip gasket is pressed against the separator;
  • FIG. 11C is an enlarged cross-sectional view of a state immediately before the gasket of the two-stage seal lip according to the first embodiment is pressed against the separator;
  • FIG. 11D is an enlarged cross-sectional view of a state where the gasket of the two-stage seal lip according to the first embodiment is pressed against the separator;
  • FIG. 11E is an enlarged cross-sectional view of a state immediately before the gasket of the two-stage seal lip according to the modified example of the first embodiment is pressed against the separator;
  • FIG. 11F is an enlarged cross-sectional view of a state in which the gasket of the two-stage seal lip according to the modification of the first embodiment is pressed against the separator.
  • FIG. 1 is a perspective view schematically showing a part of a structure of a fuel cell stack 30 as an example of a polymer electrolyte fuel cell (PEFC) according to a first embodiment of the present invention.
  • a fuel cell stack 30 includes a cell stack 20 in which a plurality of unit cell modules (cells) 1 are stacked at the center.
  • the current collecting plate 2 and the end plate 3 having a large number of inner springs 4 as an example of an elastic body are disposed on the outermost layers at both ends of the cell stack 20.
  • the four fastening bolts 7 in which the outer springs 5 are fitted into the head 7 a are connected to the end plate 3, the current collector plate 2, the cell laminate 20, the current collector plate 2, and the end from one end of the cell stack 20.
  • the nut 3 is screwed and fastened through the bolt holes 6 at the respective corners of the plate 3.
  • 60 cells 1 are stacked to form a cell stack 20, and are fastened by fastening bolts 7 and nuts 8 inserted into the bolt holes 6 as an example of fastening members.
  • the fastening member is not limited to the fastening bolt 7 and the nut 8, and may have another configuration such as a fastening band.
  • Each current collector plate 2 is disposed on both outer sides of the cell stack 20 and uses, as an example, a copper plate plated with gold so that the generated electricity can be efficiently collected.
  • the current collector plate 2 may be made of a metal material having good electrical conductivity, such as iron, stainless steel, or aluminum. Further, the surface treatment of each current collector plate 2 may be performed with tin plating, nickel plating, or the like.
  • An end plate 3 using an electrically insulating material is disposed outside each current collecting plate 2 to insulate electricity, and also serves as an insulating function.
  • the end plate 3 for example, a material manufactured by injection molding using polyphenylene sulfide resin is used.
  • Each pipe 3 a integrated with the end plate 3 is pressed against each manifold of the cell stack 20 through a gasket (not shown) that functions as an example of a manifold seal member and has a manifold through hole. It is made to communicate.
  • a gasket (not shown) that functions as an example of a manifold seal member and has a manifold through hole. It is made to communicate.
  • MEA electrolyte membrane electrode assembly
  • the outer spring 5 is disposed between the head 7a of each fastening bolt 7 and the outer surface of the end plate 3, and is adjusted at the time of assembly by a plurality of fastening bolts 7 and a plurality of nuts 8, and is fastened at, for example, 10 kN. Has been.
  • the cell 1 includes an MEA 9 having gaskets 14 as examples of sealing members on the peripheral portions of both front and back surfaces, sandwiched between a pair of conductive separators 10, specifically an anode-side separator 10A and a cathode-side separator 10C.
  • the cooling water separator 10W is arranged outside the separator, for example, the cathode side separator 10C.
  • a pair of through holes, that is, manifold holes 11 (11A, 11C, 11W) through which fuel gas, oxidant gas, and cooling water circulate are formed in the peripheral portions of the separators 10A, 10C and MEA 9. .
  • the cooling water separator 10W is provided with a pair of through-holes, that is, manifold holes 11 (11A, 11C, 11W) through which fuel gas, oxidant gas, and cooling water flow.
  • manifold holes 11 11A, 11C, 11W
  • the manifold holes 11 are stacked and communicate with each other, and the fuel gas manifold 11A, the oxidant gas manifold 11C, and the cooling water manifold 11W are independent of each other. And formed.
  • the main body portion 9a of the MEA 9 includes a polymer electrolyte membrane that selectively transports hydrogen ions, and a pair of electrode layers formed on the inner and outer surfaces of the inner portion of the polymer electrolyte membrane, that is, an anode and a cathode. It consists of an electrode layer.
  • the electrode layer has a laminated structure having a gas diffusion layer and a catalyst layer disposed between the gas diffusion layer and the polymer electrolyte membrane.
  • the anode-side separator 10A and the cathode-side separator 10C have a flat plate shape, and the surface that comes into contact with the MEA 9, that is, the inner surface has a shape corresponding to the shape of the main body 9a and the gasket 14 of the MEA 9, respectively. is doing.
  • glassy carbon (thickness 3 mm) manufactured by Tokai Carbon Co., Ltd. can be used for each of the anode side separator 10A and the cathode side separator 10C.
  • various manifold holes and bolt holes 6 penetrate each separator 10A, 10C, 10W in the thickness direction.
  • a fuel gas flow channel groove 12A and an oxidant gas flow channel groove 12C are formed on the inner surfaces of the separators 10A and 10C, respectively, and a cooling water flow is formed on the inner surface of the separator 10W (the surface on the cathode side separator 10C side).
  • a road groove 12W is formed.
  • Various manifold holes, bolt holes 6, fuel gas flow channel grooves 12A, oxidant gas flow channel grooves 12C, cooling water flow channel grooves and the like 12W are formed by cutting or molding.
  • the gaskets 14 respectively disposed on the front and back surfaces of the MEA 9 are sealing members made of an elastic body, are integrally formed with the MEA 9, and are formed on the inner surfaces of the separators 10A and 10C by pressing the MEA 9 and the separators 10A and 10C.
  • the gasket 14 is deformed according to the shape, and the outer periphery of the main body 9a of the MEA 9 and the outer periphery of the manifold hole 11 (11A, 11C, 11W) are sealed with the gasket 14 (14A, 14C, 14W).
  • FIG. 2B is a plan view showing a fuel gas gasket structure of the MEA 9 adjacent to the fuel gas flow channel 12A of the separator 10A of the fuel cell stack of FIG.
  • the space for connecting the fuel gas manifold hole 11A and the fuel gas main body 9aA, the oxidant gas manifold 11C, and the coolant manifold 11W are separated by the fuel gas gasket 14A so as to be independent of each other. is doing.
  • FIG. 2C is a plan view showing the oxidant gas gasket structure of the MEA 9 adjacent to the oxidant gas flow channel groove 12C of the separator 10C of the fuel cell stack of FIG.
  • FIG. 2D shows a plan view showing a cooling water gasket structure of the cathode separator 10C or the cooling water separator 10W of the fuel cell stack of FIG.
  • a general seal member such as a squeeze packing made of a heat resistant material is provided around various manifold holes 11. Is arranged.
  • the seal member such as the packing prevents leakage of each of the fuel gas, the oxidant gas, and the cooling water from the connecting portion between the cells 1 of the various manifold holes 11 between the adjacent cells 1.
  • FIG. 2A shows a plan view of a more specific structure of the MEA 9 of the fuel cell stack 30 in the first embodiment.
  • a frame 13 is formed on the outer periphery of the MEA 9, and a gasket 14 is formed and disposed on the outer periphery of the main body 9 a and the manifold hole 11 of the MEA 9.
  • FIG. 3B shows a partial cross section AA of the main body 9a, the frame 13 and the gasket 14 of the MEA 9.
  • FIG. 3A shows a partial cross-sectional view of the gasket structure when the MEA 109 of the conventional example is cut at the same portion
  • FIG. 3B shows a partial cross-sectional view of the structure of the gasket 14 of the first embodiment.
  • frame bodies 113 and 13 made of resin are provided on the outer periphery of the MEAs 109 and 9 by molding, and gaskets 114 and 14 are integrally formed on the upper and lower surfaces of the frame bodies 113 and 13, respectively.
  • the gaskets 114-1 and 14-1 and the gaskets 114-2 and 14-2 formed on the upper and lower surfaces of the frames 113 and 13 have the same cross-sectional shape in the vertical direction. have.
  • the gaskets 14-1 and 14-2 formed on the upper and lower surfaces of the frame 13 have the same cross-sectional shape in the upper and lower directions, but the present invention is not limited to this.
  • the upper surface is made into the conventional gasket shape, while only the lower surface is the gasket 14 of the first embodiment. It is good also as a shape.
  • the upper surface is preferably sealed by the conventional gasket 114, and when the combustible gas or the oxidant gas flows on the lower surface, the first
  • the double-seal gasket 14 of the embodiment is employed, the remarkable effect according to the first embodiment can be exerted on the lower surface where stricter sealing performance is required than the upper surface.
  • the double seal gasket shape of the application example described later in FIGS. 6A and 7A is individually arranged on the upper and lower surfaces, the effect of the double seal can be exhibited.
  • glass fiber-added polypropylene can be used as the frame body 13, and one type of olefinic thermoplastic elastomer can be used as the gasket 14.
  • a gasket material a thermosetting resin has a very high fluidity at the time of molding, and the MEA 9 electrode is impregnated. Therefore, a thermoplastic resin is preferable. Further, if each of the frame body 13 and the gasket 14 is made of a material having adhesiveness, the sealing performance is further improved.
  • FIG. 3A is a partial cross-sectional view showing the structure of a conventional gasket 114, and the seal lip 114a has a one-step mountain structure.
  • FIG. 3B is a partial cross-sectional view showing the seal structure of the first embodiment. Since the upper and lower gaskets 14-1 and 14-2 have the same shape, the upper gasket 14-1 will be described below as a representative example.
  • the gasket 14-1 formed integrally with the frame 13 is a quadrangular frame-shaped first seal formed in parallel in the plane of the MEA 9 in parallel with each side of the quadrangle that is the outer shape of the main body 9a of the MEA 9.
  • the first seal lip 15 and the second seal lip 16 are each formed in a two-step mountain shape in the vertical direction (thickness direction) of FIG. 3B. .
  • the gasket 14-1 has a first seal lip 15 disposed on the outside air side (the right side of FIG. 3B) that is raised from the surface of the frame 13. From the vicinity of the first lower peak-shaped portion 15M, the first lower peak 15B as the peak of the circular cross section of the first lower peak-shaped portion 15M, and the apex 15B of the first lower peak-shaped portion 15M The first upper mountain-shaped portion 15N of the raised second stage and the first upper vertex 15C as the vertex of the circular cross section of the first upper mountain-shaped portion 15N are formed.
  • the diameter of the bottom surface portion of the first upper mountain-shaped portion 15N is smaller than the diameter in the vicinity of the apex 15B of the first lower mountain-shaped portion 15M, and the first upper mountain-shaped portion 15N A step portion is formed at the joint with the first lower mountain-shaped portion 15M.
  • the second seal lip 16 disposed on the main body 9a side (the left side in FIG.
  • the MEA 9 also has a first lower second mountain-shaped portion 16M raised from the surface of the frame 13, A second lower peak 16B as the peak of the second lower peak-shaped part 16M, and a second upper peak-shaped part 16N of the second stage further raised from the vicinity of the peak 16B of the second lower peak-shaped part 16M, , And the second upper vertex 16C as the vertex of the second upper mountain-shaped portion 16N.
  • the diameter of the bottom surface portion of the second upper mountain-shaped portion 16N is smaller than the diameter in the vicinity of the apex 16B of the second lower mountain-shaped portion 16M, and the second upper mountain-shaped portion 16N
  • a step portion is formed at the joint with the second lower mountain-shaped portion 16M.
  • the bottom portion of the first lower mountain-shaped portion 15M and the bottom portion of the second lower mountain-shaped portion 16M are integrated to form a continuous portion 14P, and between the first and second seal lips 15, 16 Has a continuous shape.
  • the height H2 of the continuous portion 14P between the first and second seal lips 15 and 16 is set to be lower than the height H1 from the frame 13 to the separator holding position after stack assembly.
  • H1> H2 a reduction in reaction force is realized, and a double seal can be molded in a narrow range.
  • the height H2 of the continuous portion 14P is set equal to or higher than the height H1 from the frame 13 to the separator holding position after stack assembly, the height H1 of the separator holding position is set.
  • first and second seal lips 15 and 16 and the continuous portion 14P need to be elastically deformed, and the reaction force increases, resulting in a single seal instead of a double seal.
  • the interval between the first and second seal lips 15 and 16 in order to reliably achieve the double seal, the interval between the first and second seal lips 15 and 16 must be increased, and it is impossible to form a double seal in a narrow range. It becomes.
  • the heights of the first lower vertex 15B, the first upper vertex 15C, the second lower vertex 16B, and the second upper vertex 16C are the heights H1 up to the separator holding position after stack assembly. It is set higher than the upper limit so that it is deformed elastically and reliably at the time of stack assembly.
  • FIG. 10A is an enlarged cross-sectional view of a part of the gasket structure of the fuel cell stack according to the first embodiment of FIG. 3B
  • FIG. 10B is an enlarged cross-sectional view in a state where the gasket of FIG. 10A is pressed against the separator.
  • the width of the bottom surface of the lower mountain-shaped portions 15M and 16M is W
  • the width of the continuous portion 14P is d
  • the reason is as follows.
  • the reason why W> h> 0 is preferable is because of the stability of the seal lips 15 and 16. This is because when the height h is larger than the width W, the seal lips 15 and 16 are likely to become unstable.
  • the reason why W> d is preferable is that, when the width d is too large, the overall size is increased, and at the time of compression of the seal lips 15 and 16, the continuous portion 14P between the two seal lips 15 and 16 is formed.
  • the space volume of the recess 72 is increased.
  • the space volume of the recess 72 increases, the volume of water increases when the temperature of water mixed in the space of the recess 72 decreases and the water freezes.
  • the overall size is further increased and the distance between the double seal structures is further increased.
  • the water volume further increases when the water freezes.
  • the separators 10 on the upper and lower surfaces of the seal lips 15 and 16 in FIG. 10A have higher strength than the seal material, the force generated when the volume of water (water) increases is higher than that of the separator 10 or the like. It acts on the seal lips 15 and 16 and pushes the seal lips 15 and 16 in the left-right direction in FIG. 10B, so that the seal lips 15 and 16 are likely to fall down. Leakage occurs when the seal lips 15 and 16 fall. Therefore, in order to reliably prevent such a leak, it is necessary to set the dimensions so that the volume of the space of the recess 72 is minimized. For this reason, it is necessary to satisfy W> d.
  • the reason why d> 0 is preferable is that when the seal lips 15 and 16 are compressed, if the space of the recess 72 does not remain at all, when the seal lips 15 and 16 are compressed, the two seal lips 15 and 16 It pushes against each other, and the seal lips 15, 16 tend to fall down, which is not preferable.
  • the width d needs to be at least a positive value.
  • each seal lip 15, 16 is composed of a lower mountain shape portion 15M, 16M and an upper mountain shape portion 15N, 16N. The reason why the step lip (two-step mountain-shaped structure) is effective will be described.
  • the top part 114b of the one-stage mountain-shaped part 114a hits the separator 110.
  • the top portion 114b of the mountain-shaped portion 114a is crushed and compressed by elastic deformation.
  • the fastening pressure at the portion 70 where the top portion 114b of the mountain-shaped portion 114a is crushed and compressed is represented by ⁇ P and is determined by the area of the compressed portion 70 (cross-hatching). Part reference).
  • the fastening pressure indicated by the area of the cross-hatched portion is smaller in FIG. 11D of the first embodiment than in FIG. 11B of the related art. It can be clearly seen that the fastening pressure is small. Further, the peak surface pressure P MAX is substantially the same in FIGS. 11B and 11D.
  • a two-mountain type (two-step mountain-shaped structure having a plurality of upper mountain-shaped portions) as a modified example in the case of a two-step lip is a lower mountain.
  • a plurality of upper mountain-shaped portions 15N-1 and 15N-2 in the second stage further projecting from the vicinity of the vertex 15B of the shape portion 15M are provided.
  • the other seal lip 16 can also be provided.
  • the maximum value of the seal pressure resistance is that peak surface pressure P MAX higher than the gas pressure is generated at two locations where the upper mountain-shaped portions 15N-1 and 15N-2 are respectively compressed.
  • the peak surface pressure P MAX can be generated at two locations, and the sealing function can be exhibited more stably.
  • each of the peak surface pressure P MAX of the two portions of FIG. 11F is substantially the same as FIG. 11B and FIG. 11D.
  • the first seal lip 15 and the second seal lip 16 are all symmetrical with respect to the mirror upper mountain-shaped portions 15N and 16N and part of the lower mountain-shaped portions 15M and 16M.
  • the radius of curvature of the vertices is the same for the first lower vertex 15B and the second lower vertex 16B, and is the same for the first upper vertex 15C and the second upper vertex 16C.
  • the present invention is not limited to this, and different curvature radii may be used for the first upper vertex 15C and the second upper vertex 16C.
  • the correlation is R 1 ⁇ It is preferable to satisfy 0.5 ⁇ R 2 in order to achieve the effect of the present invention more reliably.
  • the curvature radius R 2 is preferably 0.2 to 0.6 mm, and in the first embodiment, 0.3 mm can be adopted as the curvature radius R 2 .
  • the first and second seal lips 15 and 16 are each composed of two ridges, and the radii of curvature R 1 and R 2 of the vertices of the two ridges are set to R 1 ⁇ 0.5 ⁇ R 2
  • the first and second seal lips 15 and 16 are elastically deformed at two locations of the first upper vertex 15C and the second upper vertex 16C, and the separator 10A or 10C is intensively sealed ( In other words, in the cross section, the sealing performance is intensively improved on the center line passing through the top of the first upper vertex 15C), and it is possible to reliably ensure the double sealing performance with a small reaction force. It becomes.
  • the curvature radius R 2 of the apex is set to R 1 ⁇ 0.5 ⁇ R 2 , not only can the shape of the gasket 14 be stably formed, but the gasket 14 can be stably formed during stack assembly. It can be fastened and it becomes possible to guarantee the sealing performance. That is, if the radius of curvature R 2 at the apex is smaller than R 1 ⁇ 0.5, the moldability deteriorates (such as a short (insufficient filling of molding resin) occurs), and at the time of stack fastening, This is because kinking occurs or a load is not applied uniformly.
  • the apex shapes of the first seal lip 15 and the second seal lip 16 are made to coincide with each other. However, if the above correlation is satisfied, the first seal lip 15 and the second seal lip Even if the 16 vertices are changed to different vertex shapes, the above-described effect is exhibited.
  • the center position of the radius R 2 is made to coincide on a straight line, depending on the internal and external environment or pressure loading conditions of the gas or water supply to the MEA 9 of MEA 9, the upper vertex 15C, the center position of the radius of curvature R 2 of 16C the lower apex 15B, with respect to the center position of the curvature radius R 1 of 16B, MEA 9 side, or, respectively the lower apex 15B to the outside air, the radius of curvature R 1 and the upper apex 15C of 16B, 16C radius of curvature R of the You may make it move within the range until 2 edge part corresponds.
  • the upper apex 15C of the second sealing lip 16 or by moving the center of the curvature radius R 2 of 16C to MEA9 side, upper vertex 15C, 16C curvature
  • the radius R 2 is set to be larger within the above range (for example, within the range of (R 1 ⁇ 0.5 ⁇ R 2 ) and the radius of curvature R 2 is close to the maximum value)
  • the second seal lip 16 caused by the internal pressure is set. This eliminates the deviation of the upper apex 16C, and is effective in improving the sealing performance when an internal pressure is applied.
  • the apex angle ⁇ of the first and second seal lips 15 and 16 is 18 ° or more, respectively. It is desirable to be.
  • the upper limit value of the apex angle ⁇ is 90 degrees from the viewpoint of surely reducing the fastening force and preventing the reduction of the surface pressure peak value of the gasket body.
  • the ratio (H / D) of the sum of the widths of both 15 and 16 is preferably H / D ⁇ 0.6. .
  • the dimension H in the thickness direction to the top of the mountain-shaped part is preferably 60% or less.
  • the lower limit of the ratio (H / D) is 0.1. This is because if the lower limit of the ratio (H / D) is less than 0.1, the sealing effect will not be improved for the increased amount of material used.
  • the optimum total width D is 0.5 to 5.0 mm.
  • the width refers to a dimension along a direction orthogonal to the thickness direction of the seal lip and orthogonal to the extending direction of the seal lip.
  • the apex angle ⁇ 18 °
  • the sealing performance may be exhibited. It will not be possible.
  • the first and second seal lips 15 and 16 are the lowest height that can exhibit the sealing performance, and can have a full width D. Since it is desirable to be as narrow as possible, it is preferable to satisfy H / D ⁇ 0.6 as described above.
  • the first and second seal lips 15 and 16 are formed in two stages, and the radius of curvature is smaller in plan and smaller in cross section than the lower ridges 15M and 16M in the first stage.
  • the upper ridge portions 15N and 16N of the second stage are arranged on the lower ridge portions 15M and 16M.
  • the upper mountain-shaped portions 15N and 16N are first brought into contact with the separators 10A and 10C during stack assembly, and are elastically deformed more easily and largely than the lower mountain-shaped portions 15M and 16M.
  • the upper mountain-shaped portions 15N and 16N function as the easily deformable portions.
  • the lower mountain-shaped portions 15M and 16M function as the enlarged portions.
  • the tops of the first and second seal lips 15 and 16 stably come into contact with the opposing surfaces of the separator 10A or 10C when a tightening load is applied during stack assembly, and elastic deformation starts. Further, it is possible to reliably prevent the first and second seal lips 15 and 16 from falling sideways, and to reliably exhibit the sealing performance.
  • the first and second seal lips 15 and 16 are brought into contact with the opposing surfaces of the separator 10A or 10C to exhibit the sealing performance, so that double sealing can be performed and the sealing performance can be reliably ensured.
  • a double seal structure can be provided. Therefore, since the sealing performance is improved as compared with the conventional case, the effect that the seal height can be made lower than that of the conventional example and the reaction force can be reduced is also exhibited.
  • the overall width D is set large, or the surface roughness of the surface of the portion of the frame 13 where the gasket 14 is molded is formed. Roughening is effective in improving the sealing performance.
  • the gasket 14 can also be formed of a resin material such as synthetic rubber, EPDM, or silicone.
  • FIG. 4A is a partial cross-sectional view of the unit cell module 1 when two gaskets 114 having a conventional shape are arranged in parallel and in contact with the separator 110 to form a double seal
  • FIG. It is a fragmentary sectional view of the cell module 1 with the gasket 14 of the shape of 1 embodiment.
  • 4A and 4B both illustrate the shape of the separator so that the shape of the seal groove of the separator can be easily understood, and do not show a cross section at the time of fastening. Therefore, the seal is shown in a state where it is not elastically deformed at all.
  • FIG. 4C shows the seal reaction force generated when a double seal is formed with the conventional gasket shape of FIG. 4A and the seal reaction force generated when the gasket shape of the first embodiment of the present invention of FIG. 4B is used. It is a graph which shows the simulation result compared.
  • the simulation was performed with general-purpose structural analysis software ABAQUS.
  • the reaction force is reduced by about 40% at the maximum as compared with the conventional example, and it is possible to realize a lower fastening pressure of the stack 30. In the experiment, the same result as the simulation was obtained.
  • the gasket 14 of the first embodiment of the present invention has a single cell configuration as compared with a double seal structure in which two gaskets 114 having a conventional shape are arranged in parallel. Since the area occupied by the gasket 14 in the module 1 is small, space can be saved and the stack 30 can be downsized.
  • FIG. 4E is a partial cross-sectional view of the unit cell module 1 when two gaskets 114 of the conventional shape of FIG. 4A are arranged in parallel and in contact with the separator 110 to form a double seal. It is a figure which shows the cross section at the time of fastening, Comprising: The seal
  • FIG. 4F is a partial cross-sectional view of the unit cell module 1 with the gasket 14 having the shape of the first embodiment shown in FIG. 4B, showing a cross-section at the time of fastening, in a state where the seal is elastically deformed.
  • FIG. 5A and FIG. 5B are diagrams respectively showing modifications of the first embodiment.
  • FIG. 5A shows a structure in which the bottom surface of the gasket 14 is buried on the frame body 13 side.
  • the recess 13a is formed in advance on the surface of the frame 13 where the gasket 14 is disposed, and the gasket 14 is fitted and disposed in the recess 13a.
  • FIG. 6A shows a partial cross-sectional view of the seal structure of the second embodiment of the present invention.
  • the first seal lip 15 on the outside air side has the same two-stage lip structure as that of the first embodiment, whereas the third seal lip 18 on the MEA side has a one-stage lip structure.
  • the 3rd seal lip 18 is good also as one mountain shape whose vertex is circular shape of a longitudinal section instead of two steps of mountain shape.
  • FIG. 6A shows the shape of the separator so that the shape of the seal groove of the separator is easy to understand, and does not show a cross-section at the time of fastening, but is a diagram of a state where the MEA and the separator are virtually assembled. For this reason, the seal is shown in a state where it is not elastically deformed at all.
  • FIG. 6B is a partial cross-sectional view of the gasket structure according to the second embodiment, showing a cross-section at the time of fastening, and a state in which the seal is elastically deformed.
  • the inside of the single cell module 1 of the fuel cell stack 30 is an atmosphere of water vapor, water, hydrogen, and oxygen, and an internal pressure of up to several hundred MPa is applied to the seal lip disposed on the MEA side.
  • the outside air is an air atmosphere, and no pressure is applied to the seal lip disposed on the outside air side.
  • the third seal lip 18 is arranged as a seal lip on the MEA 9 side instead of the second seal lip 16 of the first embodiment, the third seal lip 18 has a contact area with the separator 10A or 10C. Bigger than. For this reason, even when the internal pressures of the fuel gas and the oxidizing gas are loaded, the pressure resistance is strong, and it is possible to more reliably maintain the sealing performance for a long period of time. A higher structure can be obtained. That is, when the internal pressure on the MEA side is very large, if the shape of the third seal lip 18 is adopted, the sealing performance can be further improved in the long term. In addition, since the temperature of the unit cell module 1 rises to about 80 ° C. during startup of the fuel cell stack 30, heat resistance is also required particularly for the seal lip on the MEA 9 side. In the second embodiment, a heat-resistant thermoplastic elastomer can be used as the material of the gasket 14.
  • the inside (MEA side) is opposite to the arrangement of FIG. 6A. Even if a two-stage seal lip structure is adopted on the outside and a one-stage seal lip structure is adopted on the outside (outside air side), it is effective for improving the sealing performance and maintaining the sealing performance for a long time.
  • FIG. 7A shows a partial cross-sectional view of the seal structure of the third embodiment of the present invention.
  • This gasket 14 has a MEA 9 side second seal lip 16 having a two-step mountain structure, and the outside air side seal lip 17 is plate-shaped and has a circular and convex longitudinal section on the opposing separator 10A or 10C.
  • a convex portion 24 is formed.
  • the second seal lip 16 can maintain a reliable sealing property, and the sealing lip 17 on the outside air side and the convex portion 24 ensure the sealing property with a small fastening force. It becomes possible.
  • FIG. 7A shows the shape of the separator so that the shape of the seal groove of the separator is easy to understand, and does not show a cross-section at the time of fastening, but is a diagram of a state where the MEA and the separator are virtually assembled. In other words, the seal is illustrated in a state where it is not elastically deformed at all.
  • FIG. 7B is a partial cross-sectional view of the gasket structure according to the third embodiment, showing a cross-section at the time of fastening, and a state in which the seal is elastically deformed.
  • the polymer electrolyte fuel cell gasket of the present invention is useful as a fuel cell gasket for use in a portable power source, an electric vehicle power source, a home cogeneration system, or the like.

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PCT/JP2010/001439 2009-03-04 2010-03-03 高分子電解質型燃料電池用ガスケット Ceased WO2010100906A1 (ja)

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EP10748505.4A EP2405516B1 (de) 2009-03-04 2010-03-03 Polymerelektrolyt-brennstoffzellendichtung
JP2010546161A JP4800443B2 (ja) 2009-03-04 2010-03-03 高分子電解質型燃料電池用ガスケット
US13/254,244 US8962212B2 (en) 2009-03-04 2010-03-03 Unit cell module and gasket for polymer electrolyte fuel cell

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CN102468456A (zh) * 2010-11-17 2012-05-23 现代自动车株式会社 具有衬垫的燃料电池隔板和用于制造其的方法
US9806353B2 (en) 2010-11-17 2017-10-31 Hyundai Motor Company Fuel cell separator with gasket and method for manufacturing the same
JP2012238556A (ja) * 2011-05-13 2012-12-06 Nissan Motor Co Ltd 燃料電池
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JPWO2013171939A1 (ja) * 2012-05-17 2016-01-07 パナソニックＩｐマネジメント株式会社 燃料電池及びその製造方法
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JP2014229584A (ja) * 2013-05-27 2014-12-08 Nok株式会社 燃料電池のシール構造
US10256481B2 (en) 2015-07-13 2019-04-09 Nissan Motor Co., Ltd. Seal structure for fuel cell
WO2017009935A1 (ja) * 2015-07-13 2017-01-19 日産自動車株式会社 燃料電池のシール構造
US11005121B2 (en) 2016-10-25 2021-05-11 Toyota Jidosha Kabushiki Kaisha Gasket and fuel cell stack
CN107946515A (zh) * 2017-12-26 2018-04-20 上汽大众汽车有限公司 电池包及其密封机构
CN107946515B (zh) * 2017-12-26 2023-07-18 上汽大众汽车有限公司 电池包及其密封机构
JP2020123497A (ja) * 2019-01-30 2020-08-13 トヨタ自動車株式会社 燃料電池スタック
JP7103249B2 (ja) 2019-01-30 2022-07-20 トヨタ自動車株式会社 燃料電池スタック
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JP7196773B2 (ja) 2019-05-31 2022-12-27 トヨタ自動車株式会社 燃料電池
JP2024519448A (ja) * 2021-04-21 2024-05-14 セルセントリック・ゲーエムベーハー・ウント・コー・カーゲー 燃料電池スタック用の単セル構成体
JP7751656B2 (ja) 2021-04-21 2025-10-08 セルセントリック・ゲーエムベーハー・ウント・コー・カーゲー 燃料電池スタック用の単セル構成体
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US8962212B2 (en) 2015-02-24
US20110318665A1 (en) 2011-12-29
EP2405516B1 (de) 2014-04-30
EP2405516A1 (de) 2012-01-11
EP2405516A4 (de) 2012-11-21

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